Developing rapid detection technology for adenosine triphosphate (ATP) is crucial in quality supervision and food safety. Herein, an electrochemical aptasensor based on an aptazyme-catalyzed signal amplification strategy is constructed for ATP detection using polyethyleneimine-functionalized molybdenum disulfide (PEI-MoS2)/Au@PtPd nanobipyramids (MoS2/Au@PtPd NBPs) as a modification material. Additionally, a novel kind of nitrogen-rich covalent organic framework (COF) is prepared using melamine and cyanuric acid (MCA). We synthesize MCA and the Co-based metal organic framework (Co-MOF) as the signal label. Due to the fact that π-π stacking interactions of Co-MOF@MCA can expand the load efficiency and surface concentration of the signal label, the signal response is an order of magnitude higher than that of Co-MOF or MCA as the signal label. Target ATP changes the conformation of the aptazyme, and it becomes activated. With the assistance of metal ions, the signal label is circularly cleaved, causing an amplification of the signal. Among them, MoS2/Au@PtPd NBPs have a large specific surface area and good electrical conductivity and can carry substantial DNA strands and amplify the redox signal of methylene blue (MB). Under optimal conditions, the aptasensor can detect ATP from 10 pM to 100 μM with a low limit of detection of 7.37 × 10-10 μM. Therefore, the novel aptasensor has extensive application prospects in quality supervision and food safety.